Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 160313 - 160313
Published: Feb. 1, 2025
Language: Английский
Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 160313 - 160313
Published: Feb. 1, 2025
Language: Английский
Advanced Materials, Journal Year: 2022, Volume and Issue: 34(45)
Published: May 27, 2022
Artificial photosynthetic solar-to-chemical cycles enable an entire environment to operate in a more complex, yet effective, way perform natural photosynthesis. However, such artificial systems suffer from lack of well-established photocatalysts with the ability harvest solar spectrum and rich catalytic active-site density. Benefiting extensive experimental theoretical investigations, this bottleneck may be overcome by devising photocatalytic platform based on metal sulfides predominant electronic, physical, chemical properties. These tunable properties can endow them abundant active sites, favorable light utilization, expedited charge transportation for conversion. Here, it is described how some vital lessons extracted previous investigations are employed promote further development photosynthesis, including water splitting, CO2 reduction, N2 pollutant removal. Their functions, properties, synthetic strategies, emerging issues, design principles, intrinsic functional mechanisms redox reactions discussed detail. Finally, associated challenges prospects utilization highlighted future trends photocatalysis envisioned.
Language: Английский
Citations
262Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(44)
Published: Sept. 10, 2022
The best use of photogenerated electrons and holes is crucial to boosting photocatalytic activity. Herein, a bifunctional dual-cocatalyst-modified photocatalyst constructed based on CdS/MoO2 /MoS2 hollow spheres for hydrogen evolution coupled with selective pyruvic acid (PA) production from lactic (LA) oxidation. MoS2 MoO2 are simultaneously obtained the conversion CdMoO4 in one step. In process, function as reduction oxidation centers which accumulate used reaction (HER) PA synthesis, respectively. By monitoring intermediates, two-step single-electron route proposed, initiated by cleavage α-C(sp3 )-H bond LA. LA selectivity can reach ca. 29 % 95 after five-hour reaction,
Language: Английский
Citations
231Nature Reviews Chemistry, Journal Year: 2022, Volume and Issue: 7(2), P. 91 - 105
Published: Dec. 19, 2022
Language: Английский
Citations
163Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(29)
Published: Feb. 23, 2022
Abstract Sparked by natural photosynthesis, solar photocatalysis using metal‐free graphitic carbon nitride (g‐C 3 N 4 ) with appealing electronic structure has turned up as the most captivating technique to quest for sustainable energy generation and pollution‐free environment. Nonetheless, low‐dimensional g‐C is thwarted from sluggish kinetics rapid recombination of photogenerated carriers upon light irradiation. Among multifarious modification strategies, engineering 2D cocatalysts anticipated accelerate redox kinetics, augment active sites ameliorate electron–hole separation boosted activity thanks its face‐to‐face contact surface. It timely technological significance review 2D/2D interfaces state‐of‐the‐art cocatalysts, spanning carbon‐containing phosphorus‐containing, metal dichalcogenide, other cocatalysts. Fundamental principles each photocatalytic application will be introduced. Thereafter, recent advances cocatalyst‐mediated systems critically evaluated based on their interfacial engineering, emerging roles, impacts toward stability catalytic efficiency. Importantly, mechanistic insights into charge dynamics structure–performance relationship deciphered. Last, noteworthy research directions are prospected deliver insightful ideas future development . Overall, this serve a scaffold cornerstone in designing dimensionality‐dependent cocatalyst‐assisted renewable ecologically green
Language: Английский
Citations
140Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 455, P. 140601 - 140601
Published: Nov. 26, 2022
Language: Английский
Citations
133ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(20), P. 12823 - 12832
Published: Oct. 7, 2022
Plastic valorization presents a significantly untapped opportunity to address environmental issues while creating the necessary economic push for circular carbon economy. Compared with conventional routes processing plastics (e.g., pyrolysis and gasification), photoreforming strategy, namely, photocatalytic plastic oxidation paired water splitting, aims achieve into commodity chemicals under mild conditions offering hydrogen fuels. Here, we implement MoS2-tipped CdS nanorod photocatalysts in an aqueous medium reform pretreated that range from polyesters polylactic acid (PLA) polyethylene terephthalate (PET)) polyolefins (PE)). The architecture of MoS2/CdS takes advantage anisotropic morphology rapid charge transfer features nanorods, by collecting electrons at MoS2 tip evolution utilizing entire sidewall nanorods rich holes toward oxidation. It is shown continuous H2 can be evolved PLA, PET (commercial granules real-world bottles), PE, these substrates are accordingly converted series valuable chemicals. This work provides effective way harness solar energy realize transformation trash (plastics) treasure (gaseous/liquid chemicals).
Language: Английский
Citations
132ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(4), P. 2569 - 2580
Published: Feb. 7, 2022
Fabrication of semiconductor heterojunctions into hollow nanostructures holds multiple intrinsic advantages in enhancing the photocatalytic performance but still faces lots challenges. To overcome obstacles, herein, we report an alternative stacking design on carbon spheres for significantly improved activity, selectivity, and stability CO2-to-CO conversion. In smart design, CdS nanoparticles are first deposited then selectively coated with ZnIn2S4 outer layers, producing a ternary C/CdS@ZnIn2S4 photocatalyst. The enhancements attributed to prominent features merits carbon: (i) light reflection scattering improving harvesting; (ii) electron collection behavior promoting charge separation; (iii) large surface area increasing CO2 adsorption; (iv) highly active selective sites targeted reduction reaction; (v) porous shell spatially separating oxidation half reactions; (vi) protective layer preserving from photocorrosion; (vii) ideal architecture deposition separated redox cocatalysts. It is expected that emerging would be extended other if only two semiconductors integrated core–shell nanostructure hole-accumulated electron-accumulated core.
Language: Английский
Citations
126Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(16)
Published: Jan. 31, 2022
Abstract The photocatalytic conversion of solar energy offers a potential route to renewable energy, and its efficiency relies on effective charge separation in nanostructured photocatalysts. Understanding the charge‐separation mechanism is key improving performance this has now been enabled by advances spatially resolved surface photovoltage (SRSPV) method. In Review we highlight progress made SRSPV mapping distributions at nanoscale determining driving forces heterogeneous photocatalyst particles. We discuss how arising from built‐in electric field, diffusion, trapping can be exploited optimized through design. also importance asymmetric engineering photocatalysts for separation. Finally, provide an outlook further opportunities that arise leveraging these insights guide rational design advance imaging technique expand knowledge
Language: Английский
Citations
112Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 315, P. 121575 - 121575
Published: June 1, 2022
Language: Английский
Citations
112Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(11)
Published: Jan. 20, 2023
Electrochemical CO2 reduction reaction (CO2 RR) to chemical fuels such as formate offers a promising pathway carbon-neutral future, but its practical application is largely inhibited by the lack of effective activation molecules and pH-universal feasibility. Here, we report an electronic structure manipulation strategy electron-rich Bi nanosheets, where electrons transfer from Cu donor acceptor in bimetallic Cu-Bi, enabling RR towards with concurrent high activity, selectivity stability (acidic, neutral alkaline) electrolytes. Combined situ Raman spectra computational calculations unravel that promotes ⋅- formation activate molecules, enhance adsorption strength *OCHO intermediate up-shifted p-band center, thus leading superior activity formate. Further integration robust nanosheets into III-V-based photovoltaic solar cell results unassisted artificial leaf solar-to-formate (STF) efficiency 13.7 %.
Language: Английский
Citations
102